Composition for producing hydrogen rich water and other products

ABSTRACT

The invention provides compositions for producing hydrogen rich water, nutraceuticals, cosmetics, pharmaceuticals, and other products. In one embodiment, the invention provides a composition, e.g., a tablet, including magnesium metal, at least one water-soluble acid, and a binding agent. The magnesium metal and at least one water-soluble acid may be present in amounts sufficient to maintain a pH of less than 7, e.g., at a specific time period after reaction, and a concentration of at least 0.5 mM H 2  after reaction in 50 mL water in a container e.g., a sealed or an open container, e.g., at least 0.5 mM H 2  after reaction in 100 mL water or at least 0.5 mM H 2  after reaction in 500 mL water. The composition may also include a lubricant.

BACKGROUND OF THE INVENTION

Molecular hydrogen has been found to be of potential therapeutic use fora variety of diseases injuries. For example, H₂ has been shown to haveapplications as a method for reducing wrinkles in the skin (J.Photochem. Photobiol. B. 2012; 106:24-33), treating atopic dermatitis(Evid. Based Complement. Alternat. Med. 2013; 2013:538673), and as apost-treatment regimen for radiation therapies (Biochem. J., 2012,442(1); 49-56). Hydrogen rich water represents one way in whichmolecular hydrogen can be administered to subjects. Common electrolyticand base metal methods of producing hydrogen-rich water typically resultin an alkaline solution with a low H₂ concentration.

Creating ready-to-drink containers of H₂ (and thus hydrogen rich water)has its technical challenges. The equipment often used to saturate waterwith H₂ gas in sufficient volumes is both expensive and largelyineffective. When utilized, H₂ can be dissolved at a maximumconcentration of 0.8 mM or 1.6 ppm under SATP conditions as per Henry'slaw. In order to retain this concentration of H₂ for any period of time,the container cannot have any headspace or the drink must besupersaturated to allow H₂ dissipation into the headspace to reachequilibrium. Even when no headspace is present, the level of H₂ in thecontainer quickly falls to −1 ppm and will continue to fall towards 0ppm depending on the containment technology, level of headspace, and theinitial concentration, as seen by other commercial products on themarket. Some products retain almost no H₂ by the time they reachconsumers. For example, the Japanese government recently evaluatedconsumer goods containing H₂ and found that most had no detectable levelof H₂ present. (httpwww.kokusen.go.jp/news/data/n-20161215_2.html).

Accordingly, there is a need for new compositions for producinghydrogen-rich water which maximize the dissolved hydrogen concentration.

SUMMARY OF THE INVENTION

The invention provides compositions for producing hydrogen rich water,nutraceuticals, cosmetics, pharmaceuticals, and other products. In oneembodiment, the invention provides a composition, e.g., a tablet,including magnesium metal, at least one water-soluble acid, and abinding agent. The magnesium metal and at least one water-soluble acidmay be present in amounts sufficient to maintain a pH of less than 7,e.g., at a specific time period after reaction, and a concentration ofat least 0.5 mM H₂ after reaction in 50 mL water in a container e.g., asealed or an open container, e.g., at least 0.5 mM H₂ after reaction in100 mL water or at least 0.5 mM H₂ after reaction in 500 mL water. Thecomposition may also include a lubricant.

In another aspect, the invention provides a composition containingmagnesium metal, at least one water-soluble acid, and a binding agent,where the at least one water-soluble acid has a solubility of at least0.01 g/mL in water. In certain embodiments, the compositiondisintegrates in less than 5 minutes, in particular less than 2 minutes.In certain embodiments, the composition produces at least 0.5 mM H₂after contact with 50 mL water in a container at atmospheric pressureand room temperature, e.g., at least 0.5 mM H₂ after reaction in 100 mLwater or at least 0.5 mM H₂ after reaction in 500 mL water. Thecomposition may also include a lubricant.

In certain embodiments of the above aspects, the compositiondisintegrates in less than 5 minutes, e.g., in less than 2 minutes. Incertain embodiments, the disintegrated composition maintains a pH ofless than 7 at 10 minutes after being contacted with water and producesat least 0.5 mM H₂ after contact with 50 mL water in a container atatmospheric pressure and room temperature, e.g., at least 0.5 mM H₂after reaction in 100 mL water or at least 0.5 mM H₂ after reaction in500 mL water.

In another aspect, the invention provides a composition containingmagnesium metal, at least one acid, and a binding agent where thecomposition disintegrates in less than 5 minutes to maintain a pH ofless than 7 10 minutes after disintegration and at least 0.5 mM H₂ aftercontact with 50 mL water in a container at atmospheric pressure and roomtemperature, e.g., at least 0.5 mM H₂ after reaction in 100 mL water orat least 0.5 mM H₂ after reaction in 500 mL water.

In certain embodiments of any of the above aspects, the compositionpasses a pharmaceutical test for friability. In certain embodiments, thepH of the water is less than 7 at 10, 15, 20, 30, or 45 minutes afterthe composition is contacted with water. In certain embodiments, the pHof the water is less than 7 at least 1 hour after the composition iscontacted with water. In certain embodiments, the container is open tothe atmosphere. In certain embodiments, the container is closed. Incertain embodiments, when the container is closed the pH remains lessthan 7 at 7 days after contact with water. In certain embodiments, themagnesium in the composition reacts to produce H₂ as it disintegrates inwater, i.e., that rate of disintegration and rate of consumption ofmagnesium are substantially the same.

The amount of magnesium metal is, for example, 5-500 mg, e.g., 5-100 mg.The amount of acid is, for example, 30-4000 mg, e.g., 200-400 mg. Incertain embodiments, the magnesium metal and acid are present in amountssufficient to maintain a pH of between 4 and 6, and/or the magnesiummetal and acid are present in amounts sufficient to produce aconcentration of at least 2 mM H₂ in 50 mL of water in a container,e.g., a sealed or an open container, e.g., at least 2 mM H₂ afterreaction in 100 mL water or at least 2 mM H₂ after reaction in 500 mLwater. In certain embodiments, the magnesium metal includes flakes,e.g., −325 mesh flakes. In other embodiments, the magnesium metal iscrushed, e.g., of 200 mesh or smaller. In some embodiments, the at leastone acid is an edible acid. The edible acid is, for example, maleicacid, succinic acid, malic acid, fumaric acid, formic acid, citric acid,ascorbic acid, oxalic acid, tartaric acid, or a combination thereof.Exemplary edible acids are tartaric acid and malic acid. In someembodiments, the acid is a cosmetically or pharmaceutically acceptableacid. The cosmetically or pharmaceutically acceptable is, for example,acetic acid, adipic acid, alginic acid, aspartic acid, benzenesulfonicacid, benzoic acid, boric acid, butyric acid, camphoric acid,camphersulfonic acid, cyclopentanepropionic acid, digluconic acid,dodecylsulfric acid, ethanesulfonic acid, glucoheptonic acid,glycerophosphoric acid, hemisulfuric acid, heptonic acid, hexanoic acid,hydrobromic, hydrochloric acid, hydroiodiic acid,2-hydroxy-ethanesulfonic acid, lactobionic acid, lactic acid, lauricacid, lauryl sulfuric acid, malonic acid, methanesulfonic acid,2-naphthalenesulfonic acid, nicotinic acid, nitric acid, oleic acid,palmitic acid, pamoic acid, pectic acid, persulfuric acid,3-phenylpropionic acid, phosphoric acid, picric acid, pivalic acid,propionic acid, stearic acid, sulfuric acid, tartric acid, thiocyanicacid, toluenesulfonic acid, undecanoic acid, valeric acid, or acombination thereof. Other acids include acetylsalicylic acid and5-aminosalicylic acid. Examples of binding agents are mannitol, xylitol,maltose, dextrose, and lactose. Exemplary binding agents are dextroseand lactose. In certain embodiments, when the acid is tartaric citric,or ascorbic acid, the amount of magnesium is greater than 20 mg, e.g.,at least 50 mg, or when the acid is acetylsalicylic acid and5-aminosalicylic acid, the amount of magnesium is greater than 20 mg,e.g., at least 50 mg.

The composition may further include a nutritional supplement, e.g., amagnesium salt, sweetener, flavoring agent, coloring agent, fragrance,essential oil, water-soluble lubricant, or polysaccharide. Exemplarypolysaccharides include cellulose and its derivatives, e.g., methylcellulose or hydroxypropyl methyl cellulose, starch, apple powder, lemonpowder, lime powder, grapefruit powder, psyllium husk, and pectin.Exemplary lubricants include sodium stearyl fumarate and stearic acid,in particular sodium stearyl fumarate.

The invention also provides a kit including a composition of theinvention and a sealable container capable of holding between 100 mL and2 L of water, e.g., between 150-750 mL of water. In certain embodiments,the container is double walled.

The invention further provides a method of producing hydrogen rich waterby contacting a composition of the invention with water in a containerso that the composition disintegrates and the magnesium metal and atleast one acid react, e.g., to produce H₂ in the water at aconcentration of at least 0.5 mM H₂ and maintain a pH of less than 7 at10 minutes after disintegration at atmospheric pressure and roomtemperature. In certain embodiments, the water includes fruit juice,e.g., a juice containing pectin. In other embodiments, the concentrationof H₂ is at least 1 mM. In certain embodiments, a pH of less than 7 ispresent at 1 hour after disintegration.

The invention further provides a method of administering hydrogen to asubject by providing the subject with a composition containing hydrogenproduced from a composition of the invention, e.g., a tablet. In someembodiments, the composition containing hydrogen is a nutraceutical ortopical formulation. In one embodiment, the nutraceutical is a beverage.

The invention further provides compositions enriched with hydrogen withthe hydrogen gas dissolved in a carrier at a concentration of at least0.5 mM, e.g., at a pH of less than 7. In some embodiments, the carrieris edible, cosmetic, or pharmaceutical grade. In some embodiments, thecarrier is an aqueous liquid, cream, lotion, foam, paste, or gel. Insome embodiments, the composition is a beverage. In certain embodiments,the maximum concentration of hydrogen is 20 mM. In some embodiments, thecomposition has a pH of 4-6. In one embodiment, the pH is 4.6 or lower.In some embodiments, the composition contains a nutritional supplement.In one embodiment, the nutritional supplement contains magnesium ions,potassium ions, or calcium ions. In some embodiments, the compositioncontains a sweetener, flavoring agent, coloring agent, fragrance,essential oil, or polysaccharide. In some embodiments, the compositioncontains a binding agent or water-soluble lubricant.

The invention further provides compositions for producing acidichydrogen rich water. In one embodiment, the invention provides acomposition, e.g., a tablet, including magnesium metal, an edible acid,and a binding agent. In general, the magnesium metal and edible acid arepresent in amounts sufficient to produce a pH of less than 7 and atleast 0.5 mM H₂ after reaction in 500 mL of water in a sealed container.The invention also provides a kit including this composition of theinvention, e.g., a tablet, and a sealable container capable of holdingbetween 200 mL and 2 L of water, e.g., between 250-750 mL of water. Incertain embodiments, the container is double walled. The inventionfurther provides a method of producing hydrogen rich water by contactingthis composition of the invention, e.g., a tablet, with water in asealable container so that the composition, e.g., tablet, disintegratesand the magnesium metal and acid react to produce H₂ in the water at aconcentration of at least 0.5 mM H₂ and a pH of less than 7, e.g.,between pH is 4-6. In certain embodiments, the water comprises fruitjuice, e.g., a juice containing pectin. In other embodiments, theconcentration of H₂ is at least 1 mM. The amount of magnesium metal is,for example, 5-100 mg. In certain embodiments, the magnesium metal andedible acid are present in amounts sufficient to produce a pH of between4 and 6, and/or the magnesium metal and edible acid are present inamounts sufficient to produce at least 2 mM H₂ in 500 mL of water in thesealed container. In certain embodiments, the magnesium metal ispowdered, e.g., of 200 mesh or smaller. In other embodiments, themagnesium metal includes flakes, e.g., −325 mesh flakes. The edible acidis for example, selected from the group consisting of maleic acid,succinic acid, malic acid, fumaric acid, formic acid, citric acid,ascorbic acid, and oxalic acid. Examples of binding agents are mannitol,xylitol, maltose, and lactose. The composition may further include avitamin, mineral, e.g., a magnesium salt, sweetener, flavoring agent,water soluble lubricant, or polysaccharide. Exemplary polysaccharidesinclude methyl cellulose, starch, apple powder, lemon powder, limepowder, grapefruit powder, psyllium husk, and pectin.

Definitions

As used herein, the term “cosmetic” refers to a composition that isapplied to the all or a part of the human body, e.g., hands, face, arms,or legs, for cleansing, beautifying, promoting attractiveness, oraltering the appearance.

As used herein, the term “cosmetically acceptable” refers to acomposition having ingredients which are acceptable for human topicaluse.

As used herein, the term “nutraceutical” refers to a composition havingingredients suitable at least for human consumption. Pharmaceuticalgrade ingredients may optionally be employed, as described in, e.g.,“Remington: The Science and Practice of Pharmacy” (22nd ed.), ed. L. V.Allen, Jr., 2013, Pharmaceutical Press, Philadelphia, Pa.

As used herein, the term “passes a pharmaceutical test of friability”refers a composition that decreases in mass by at most 1% after 100revolutions in a rotating drum of a friability tester, e.g., from CopleyScientific.

As used herein, the term “pharmaceutically acceptable” refers to acomposition having ingredients which are subject to the U.S. Food andDrug Administration's pharmaceutical purity standards and furtherregulated by standards set by the U.S. Pharmacopoeia; this standard is99.9% purity of a particular ingredient.

As used herein, the term “subject” refers to any animal capable of beingtreated topically, orally, inhalation, or intravenously with acomposition containing or used to generate H₂. Animals include fish,reptiles, birds (e.g., chicken, turkey), and mammals. Mammals capable ofbeing treated with compositions of the invention include primates (e.g.,humans, apes), livestock (e.g., cows, pigs, sheep), beasts of burden(e.g., ox, horse, llama), and companion animals (e.g., dogs, cats).

DETAILED DESCRIPTION OF THE INVENTION

The present invention provides a composition, e.g., a tablet, thatdisintegrates in water to produce hydrogen rich water. By using acomposition of the invention, e.g., in a ready-to-drink container,supersaturated levels of H₂ can be achieved, considerably more than canbe achieved by addition of pure H₂ gas. In contrast to priorcompositions, an advantage of the present invention is the ability toproduce a hydrogen-enriched composition that contains a supersaturatedamount of H₂ in an open container, i.e., at atmospheric pressure. Inaddition, the present invention provides compositions that pass apharmaceutical friability test but still produce high levels of H₂. Afurther advantage of the invention is that the compositions can reactquickly, e.g., in less than 2 minutes, to produce a usable, e.g.,drinkable, hydrogen-enriched product having H₂ levels significantlyhigher than prior compositions.

The composition contains magnesium metal, i.e., elemental magnesium, anacid, and typically a binding agent and/or a lubricant. In water or awater-containing carrier, the magnesium metal and acid react to produceH₂, which dissolves in the water, and magnesium ions. An advantage ofthe present invention is that the composition contains sufficient acidto maintain an acidic pH during H₂ production. When insufficient acid isemployed, the pH of the reaction will increase, e.g., until the solutionis alkaline, causing the reaction to cease prior to reaching high levelsof H₂. Without wishing to be bound by theory, at high pH, the productionof H₂ ceases due to passivation from hydroxides and carbonates acting asligands with the unreacted magnesium particles. When this occurs, lessof the magnesium metal will react, thereby reducing the available H₂produced while leaving unacceptable levels of residual solids from thecomposition behind in the container. Use of an acid is alsoadvantageous, as a low pH, e.g., 4.6 or lower, aids in reducingmicrobial growth and therefore reducing the possibility ofcontamination. Thus, in certain embodiments, the invention providescompositions that produce a hydrogen-enriched product having an acidicpH during use or storage.

Magnesium Metal

Each composition contains a sufficient mass of magnesium to produce asufficient volume of H₂ in the volume of water to which it is added.Accordingly, in certain embodiments, the composition contains asufficient mass of magnesium to produce at least 0.1 mmol of H₂, e.g.,at least 0.5 mmol, 1 mmol, 2 mmol, 3 mmol, 5 mmol, or 10 mmol of H₂, forexample in at least 50, 75, 100, 125, 150, 175, 200, 225, 250, 500, 750,1000, 1500, or 2000 mL of a suitable carrier, e.g. water. Suitablemasses of magnesium metal include 5-1000 mg, e.g., 5-500 mg, 5-450 mg,10-400 mg, 20-350 mg, 30-300, 40-250 mg, 50-200 mg, 60-100 mg, or about70 mg or 80 mg of magnesium.

The physical form, e.g., size and shape, of the magnesium may be used tocontrol the rate of reaction. Particles may be spherical, spheroidal,granular, or flaked. Smaller particles and particles with higher surfacearea to volume ratios react with faster kinetics. Mixtures of varioussizes may also be employed. Flaked magnesium has a higher surface areato volume ratio than granular magnesium. In certain embodiments, flakedmagnesium of −325 mesh may be employed in the composition.Alternatively, or in combination, larger sized magnesium or magnesiumwith a lower surface area to volume ratio relative to flaked magnesiummay be employed. For example, magnesium of −200 mesh may be employed. Inother embodiments, magnesium of +100, −100, +200, −200 (e.g., −200,+325), −325, or smaller mesh is employed. In certain embodiments, themagnesium is supplied in two sizes, e.g., −200 and −325, with thesmaller size being 20-50% of the total and the larger size being thebalance.

Acids

Any water-soluble acid may be employed in the invention. The acid may beedible, or otherwise of cosmetic or pharmaceutical grade. Examples ofedible acids include, but are not limited to, maleic acid, succinicacid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid,oxalic acid, tartaric acid, and combinations thereof. Examples ofcosmetic or pharmaceutical grade acids include acetic acid, adipic acid,alginic acid, aspartic acid, benzenesulfonic acid, benzoic acid, boricacid, butyric acid, camphoric acid, camphersulfonic acid,cyclopentanepropionic acid, digluconic acid, dodecylsulfric acid,ethanesulfonic acid, glucoheptonic acid, glycerophosphoric acid,hemisulfuric acid, heptonic acid, hexanoic acid, hydrobromic,hydrochloric acid, hydroiodiic acid, 2-hydroxy-ethanesulfonic acid,lactobionic acid, lactic acid, lauric acid, lauryl sulfuric acid,malonic acid, methanesulfonic acid, 2-naphthalenesulfonic acid,nicotinic acid, nitric acid, oleic acid, palmitic acid, pamoic acid,pectic acid, persulfuric acid, 3-phenylpropionic acid, phosphoric acid,picric acid, pivalic acid, propionic acid, stearic acid, sulfuric acid,tartric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid,valeric acid, their stereoisomers, all forms of alpha acids (e.g.,α-lupulic acid), polycarboxylic acids, a Lewis acid, e.g., AlCl₃, andcombinations thereof. Other acids include acetylsalicylic acid and5-aminosalicylic acid. The acid will be present in an amount to reactwith the magnesium metal and optionally to maintain a pH of less than 7when the composition is placed in water. It is preferable that theamount of acid chosen is sufficient to maintain a pH of less than 6,e.g., between 4 and 6, for the duration of typical beverage consumptione.g., at least 30 minutes or 1 hour. In certain embodiments, the numberof moles of acid protons in the acid is at least 10, 20, 30, 40, 50, 75,or 100% greater than the number of moles of magnesium metal present.Suitable masses of the acid include 30-4000 mg, e.g., 100-1000 mg,50-900 mg, 100-800 mg, 150-700 mg, 200-600 mg, 250-500 mg, 300-400 mg,or about 340 mg of acid. An exemplary edible acid is malic acid. Anotherexemplary edible acid for use in compositions of the invention istartaric acid. Tartaric acid is highly water-soluble, having asolubility of 0.125 g/mL in water. Acids with a solubility of betweenabout 0.01-1 g/mL, e.g., between about 0.02-0.9 g/mL, between about0.03-0.8 g/mL, between about 0.04-0.7 g/mL, between about 0.05-0.6 g/mL,between about 0.06-0.5 g/mL, between about 0.07-0.4 g/mL, between about0.08-0.3 g/mL, between about 0.09-0.2 g/mL, between about 0.1-0.2 g/mL,between about 0.11-0.5 g/mL, or between about 0.12-0.3 g/mL, aresuitable for use in compositions of the invention. When highlywater-soluble acids are used in a composition of the invention, thecomposition is able to quickly disintegrate upon contact with water,e.g., resulting in a more complete reaction with magnesium. This fastdissolution has the benefit of allowing the pH to remain below 7 on atimescale commensurate with beverage consumption, e.g., 1-2 hours. Othersuch acids, both edible and cosmetic and/or pharmaceutical grade, areknown in the art.

The physical form, e.g., size and shape, of the acid may be used tocontrol the rate of the reaction. For example, acids that are solids atroom temperature, e.g., malic acid or tartaric acid, can be processed tocontrol the size of the acid particles used to produce a composition ofthe invention. Smaller particles and particles with higher surface areato volume ratios react with faster kinetics. Milled acid particles maybe used in a variety of mesh sizes, e.g., 40 mesh through 2500 mesh.Without being bound by theory, the rate of the dissolution of thecomposition is believed to be linearly dependent on mesh size.Compositions of the invention made with larger acid particles, e.g.,40-60 mesh, dissolve more slowly than those made with finer, e.g., 120mesh through 2500 mesh acid particles. Mixtures of various sizes of acidparticles may also be employed. Acid particles with controllable sizesmay be produced by a number of different techniques, including, but notlimited to, micronizing, ball milling, or tumbling. Other methods ofproducing acid particles with controllable sizes are known in the art.

Binding Agents

Any binding agent capable of disintegrating in water may be employed.Examples of binding agents include sugars such as maltose, dextrose, andlactose, and sugar alcohols such as mannitol and xylitol. Exemplarybinding agents for compositions of the invention include lactose anddextrose. Other binding agents for compositions are known in the art.The amount of binding agent is, for example, between 10 and 50% of theweight of the composition, e.g., between 20-30%. Compositions of theinvention may include a single binding agent, such as lactose, or may bemade from a combination of two or more binding agents to control thephysical properties of the composition.

The binding agent may be edible, or otherwise be of cosmetic orpharmaceutical grade as is known in the art, e.g., in Remington(Remington: The Science and Practice of Pharmacy, (22nd ed.) ed. L. V.Allen, Jr., 2013, Pharmaceutical Press, Philadelphia, Pa.).

Additional Components

The composition may also include other ingredients such as a nutritionalsupplement, sweetener, flavoring agent, coloring agent, fragrance,essential oil, lubricant, polysaccharide, or coating. Compositions ofthe invention may contain nutritional supplements, e.g., vitamins,minerals, and/or herbal extracts. For example, the composition maycontain a magnesium, potassium, or calcium salt. Suitable sweeteners areknown in the art, e.g., sucrose, mannose, sucralose, aspartame,saccharin, stevia, monk fruit extract, and acesulfame K. The compositionmay also include any food grade coloring, e.g., FD&C dyes, and/orflavoring, such as a fruit flavoring. The composition may furtherinclude an essential oil, e.g., grapeseed oil, oil of wintergreen,lavender oil. Other essential oils are known in the art. A compositionmay further include a fragrance, e.g. eucalyptus. A composition may alsocontain a polysaccharide, such as pectin, psyllium fiber, cellulose, andits derivatives, e.g., methyl cellulose or hydroxypropyl methylcellulose, various starches, apple powder, lemon powder, lime powder, orgrapefruit powder. Polysaccharides may increase the amount of H₂retained after reaction. A composition may further include awater-soluble lubricant such as micronized sodium stearyl fumarate orfinely prepared stearic acid, e.g., 5 micron. The composition may alsohave a water-penetrable coating, such as a soluble surfactant, tocontrol the rate at which the composition dissolves. The solublesurfactant coating may be a triblock co-polymer, e.g., a poloxamer,e.g., Poloxamer 407, or a non-ionic polymer surfactant suitable forpharmaceutical use, e.g., glucosides. For example, the composition mayhave a coating that dissolves in under 5 minutes, e.g., under 1 minute,to allow the user to close a container before the composition begins todisintegrate and H₂ production begins.

Previous attempts to produce effervescent compositions, e.g., tablets,using typical lubricants such as sodium lauryl sulfate as described inU.S. Patent Publication 2016/0113865, and sodium stearyl fumarate,proved unsuccessful in producing tablets that rapidly disintegrated.This was due to the use of a higher amount of lubricant needed to formthe tablets. The use of large quantities of non-micronized lubricantresulted in a tablet which had a slow disintegration time, which furthercreated excess undissolved residues in a container and a foul taste. Incontrast, compositions of the invention can make use of much lesslubricant, resulting in faster reaction kinetics, a satisfactory amountof residue, and a palatable taste.

Forms of Composition

The composition may be formed into a tablet. A tablet may be of anysuitable shape. For example, the tablet may be a disk, a sphere, or anovoid. A single tablet will typically include the amount of magnesiumand acid required to produce the desired amount of H₂ in a given volumeof water, e.g., 50, 150, or 500 mL. However, a combination of multiple,smaller tablets may be employed. For example, tablets may be sized toprovide sufficient H₂ in 250 mL, and multiple tablets may be employedfor larger volumes. As the reaction of magnesium metal and acid isactivated by water, the compositions of the invention will typically bestored in water-resistant packaging, such as foil or plastic. Thecomponents of the tablet will typically also be non-hygroscopic, buthygroscopic ingredients may be employed if the tablet is packaged dry ina waterproof container or wrapper. Tablets may be formed by methodsknown in the art.

A consideration when forming compositions of the invention into tabletsis the tablet physical properties, e.g., friability. Friability isdefined as the tendency for a tablet to chip, crumble or break followingcompression or other handling. Friability of tablets is assessed using arotating drum and measuring the percent mass loss of tablets afterrolling around the drum for a fixed number of drum revolutions. For atablet to successfully pass friability testing, the tablet's mass canonly decrease by 1% after 100 revolutions in the rotating drum. Forcompositions of the invention, friability is controlled by the type andgrain size of acid used in the composition, the type and grain size ofthe binding agent, type and grain size of the lubricant, and thepressure at which the tablets were pressed in the die. The use of morefinely meshed particles typically results in tablets that are highlyfriable. As a result of this, tablets made of finely meshed particlesare often made under higher pressure to ensure they do not fall apart;this has the effect of making the tablet very hard, reducing the speedat which it can disintegrate upon contact with water. Thus, tabletsusing fine mesh acid may be made of a highly water-soluble acid, such astartaric acid, in order to sustain the hydrogen generation reaction.

Other forms of the composition may also be employed. For example, thecomposition may be provided in the form of a powder, e.g., inside awater-soluble capsule or water-permeable bag, or small or large beads,e.g., a bath bomb, or a film.

The dissolution time of the composition, and thus the measuredconcentration of H₂, is controlled by the percent mass of the bindingagent, the percent mass and type of lubricant, the acid to magnesiumratio, the physical properties of both the magnesium and the acid, e.g.,mesh size and the physical conditions the composition is placed in.Compositions of the invention will typically disintegrate when contactedwith water in a container in less than 5 minutes, e.g., less than 4minutes, less than 3 minutes, less than 2 minutes, or less than 1minute.

The temperature of the water the composition is placed in affects howquickly the composition disintegrates. Hot water will cause thecomposition to disintegrate quickly, but not hold a high concentrationof hydrogen gas. Colder water increases the solubility of hydrogen inwater, but does not cause rapid disintegration of the composition. Asuitable temperature for the production of hydrogen from a compositionof the invention is approximately room temperature, e.g., between 15°C.-25° C., e.g., 15° C., 16° C., 17° C., 18° C., 19° C., 20° C., 21° C.,22° C., 23° C., 24° C., or 25° C., e.g., between 59° F.-77° F., e.g.,59° F., 60° F. 61° F., 62° F., 63° F., 64° F., 65° F., 66° F., 67° F.,68° F., 69° F., 70° F., 71° F., 72° F., 73° F., 74° F., 75° F., 76° F.,or 77° F.

The compositions will maintain an acidic hydrogen-enriched product,e.g., having a pH less than 7, e.g., 4-6, for at least a period of timeafter being contacted with water. An acidic pH may be maintainedthroughout the course of the typical time scale for use of thehydrogen-enriched product, such as 10 minutes after the composition iscontacted by water. For example. the composition of the inventionmaintains a pH of less than 7 for a period of time of at least 5minutes, e.g., 5-300 minutes, 10-250 minutes, 15-200 minutes, 20-150minutes, 25-120 minutes, 30-100 minutes, 50-90 minutes, e.g., at least 5minutes, at least 10 minutes, at least 15 minutes, at least 20 minutes,at least 25 minutes, at least 30 minutes, at least 35 minutes, at least40 minutes, at least 45 minutes, at least 50 minutes, at least 55minutes, at least 60 minutes, at least 70 minutes, at least 80 minutes,at least 90 minutes, at least 100 minutes, at least 110 minutes, atleast 120 minutes, at least 130 minutes, at least 140 minutes, at least150 minutes, at least 160 minutes, at least 170 minutes, at least 180minutes, at least 190 minutes, at least 200 minutes, at least 250minutes, or at least 300 minutes, e.g., at least 0.5 hours, at least 1hour, at least 1.5 hours, at least 2 hours, at least 2.5 hours, at least3 hours, at least at least 3.5 hours, at least 4 hours, at least 4.5hours, or at least 5 hours. Compositions may also maintain a pH that isless than 7 for an extended period of time, e.g., at one day, sevendays, 30 days, or 6 months after the composition is contacted withwater. Furthermore, after this timeframe, the pH of the hydrogenenriched product may become alkaline, e.g., greater than 7.

For compositions designed for use as a cosmetic additive to a shower orbath, the rate of dissolution of the tablet is an importantconsideration. The composition has to dissolve slowly enough in thewater in order to produce a consistent level of H₂ for the duration ofthe time in the shower or bath. An additional constraint is thethermodynamics of the dissolution reaction, as the reaction isexothermic and produces small amounts of magnesium hydroxide. If thereaction proceeds too quickly, the temperature of the resulting bathcould become too hot or produce too much magnesium hydroxide; both ofthese effects can harm the skin. The addition of polysaccharides to thecompositions has been shown to have an effect on the dissolution ratewhile maximizing retained H₂. The added polysaccharide can be a fibrouspolysaccharide, such as cellulose and its derivatives, e.g.,hydroxypropyl methylcellulose (HPMC, known as hypromellose).Alternatively or additionally, the addition of a soluble surfactant,such as a triblock co-polymer (e.g., Poloxamer 407) can be used to slowdown the dissolution of the tablet, ensuring sufficient consumption ofthe magnesium and maximizing the length of time that H₂ is dissolved inthe water.

Liquids enriched with hydrogen for use as a cosmetic or beauty spray canhave a larger acid content, and the resulting composition can takeadvantage of the skin's naturally occurring pH of 4.5-5.2 (Lambers etal., Int. J. Cosmet. Sci., 2006, 28, 359-370) to further enhance the H₂concentration. H₂ has been shown to provide numerous benefits to theskin, and using the beauty spray as a cleanser to return the skin to itsnatural pH may have further health benefits.

Carriers

Compositions of the invention, e.g., tablets, are used by contactingthem with a carrier such as water or other aqueous liquid. The water maybe pure, e.g., deionized, or may contain other dissolved ions, e.g.,spring or tap water. The water may also contain other ingredients, e.g.,it can be or contain fruit juice, or may contain other dissolved gases,e.g., carbonated water, or dissolved solids, e.g., table sugar or salt.An exemplary fruit juice is lemon juice.

The volume of carrier is selected based on the application to beenriched with hydrogen. When a composition of the invention is used toproduce a beverage, the volume of liquid, e.g., water or fruit juice, tobe enriched is from about 100 mL to 2 L, e.g., about 100 mL, about 150mL, about 200 mL, about 250 mL, about 300 mL, about 350 mL, about 400mL, about 450 mL, about 500 mL, about 550 mL, about 600 mL, about 650mL, about 700 mL, about 750 mL, about 800 mL, about 850 mL, about 900mL, about 950 mL, about 1 L, about 1.5 L, or about 2 L. When acomposition of the invention is used to produce a cosmetic product, theamount of water is from about 50 mL to 500 mL, e.g., about 50 mL, about100 mL, about 150 mL, about 200 mL, about 250 mL, about 300 mL, about350 mL, about 400 mL, about 450 mL, or about 500 mL.

Alternatively, the water may be present in a topical carrier such as acream, lotion, foam, paste, or gel such that H₂ can be effectivelydelivered to the skin. Methods of producing water-soluble topicalcarriers are well-known in the art, e.g., as described in Remington(Remington: The Science and Practice of Pharmacy, (22nd ed.) ed. L. V.Allen, Jr., 2013, Pharmaceutical Press, Philadelphia, Pa.) and in thecosmetics industry. During or after reaction of the composition of theinvention with water, the carrier can be stirred, mixed, or agitated toensure uniform consistency.

Containers

Various containers may be used to contact the composition with a volumeof water. In one embodiment, the container has a lid that may be used toseal the container, e.g., shortly after introducing a composition into avolume of water. A sealed container retains H₂ produced while thereaction proceeds to completion. Alternatively, H₂ can be produced in anopen container. An example of a suitable container is a double walled,double gasketed stainless steel bottle.

Methods of Use

Compositions of the invention, e.g., tablets, are used by contactingthem with a carrier that facilitates the dissolution of the composition.An exemplary carrier is water. Typically, the amount of water used todissolve the composition is between 50 mL and 2 L, e.g., 50 mL, 150 mL,250 mL, 355 mL, 500 mL, 750 mL, or 1 L. The user can add the compositionto the water or other carrier in a sealable container and allow thereaction to proceed for 1 or more minutes depending on the temperatureof the water, e.g., 1-2 minutes, at least 5 min, 10 min, 15 min, 30 min,45 min, 60 min, 90 min, or 12 h. In certain embodiments, it is preferredthat the composition react in less than 2 minutes. Preferably, thetablet and volume of water produce a concentration of at least 0.5 mM,e.g., at least 1 mM, at least 3 mM, at least 5 mM, or at least 10 mM,e.g., between 0.5-20 mM, 1-15 mM, or 5-10 mM. The inclusion of apolysaccharide, either in the composition, or in the water or carrier,e.g., in fruit juice, may increase the concentration of H₂ relative tothe reaction in the absence of the polysaccharide, either locally nearthe polysaccharide or in the H₂ enriched composition as a whole.

As is known in the art, the consumption of hydrogen rich water aids inthe treatment of various disorders including Parkinson's disease(Yoritaka et al., BMC Neurology, 2016, 16:66), depression (Zhang et al.Sci. Rep. 2016; 6:23742), periodontitis (Azuma et al. Antioxidants(Basel). 2015; 4(3):513-22), diabetes type II, metabolic syndrome,chronic renal failure, inflammation, rheumatoid arthritis, interstitialcystitis, cerebral ischemia, hyperlipidemia, chronic hepatitis B, andothers as described in Ichihara et al. (Med. Gas Res. (2015) 5:12).Accordingly, the compositions of the present invention may be consumedby subjects suffering from any of these disorders to treat the disorderor alleviate one or more symptoms thereof.

Additionally, H₂ has been shown to be an effective treatment for avariety of dermatological conditions. For example, when a composition ofthe invention is used to make a hydrogen enriched aqueous liquid, the pHof the resulting aqueous liquid can be adjusted to create a “beautywater” with a pH of 4.5-5.5, which has numerous health benefits (Lamberset al., Int. J. Cosmet. Sci. 2006, 28, 359-370). This “beauty water” hasbeen used as a carrier base for ionic magnesium topical cosmetics, withthe lower pH and H₂ content effectively facilitating magnesiumabsorption through the skin (Magnes. Res. 2016; 29(2):35-42). In anotherexample, H₂ containing products have been shown to be a promisingtreatment for topical skin conditions such as wrinkles, atopicdermatitis, and UV-induced burns to the skin (Mol. Cell. Toxicol. 2013,9(1), 15-21). For topical indications, the compositions of the inventioncan be directly incorporated into a dermatological carrier such as acream, lotion, foam, paste, or gel.

Hydrogen containing products produced from in-situ generation of H₂ canbe used to improve the health of certain livestock animals, inparticular, dairy cows. It is believed that H₂ has potential to increasethe usable lifespan and longevity of dairy cows, resulting in increasedmilk production.

Compositions of the invention may also be used to produce hydrogen gasthat is inhaled, e.g., by breathing the gas as it evolves either from anopen container or via a cannula or nasal tube.

Hydrogen-Enriched Acidic Compositions

A composition of the invention can be used in the manufacture of anumber of consumer products, including, but not limited to, ediblefoodstuffs and nutraceuticals (e.g., beverages), and skin care products,e.g., lotions, bath bombs, or shower tablets, for effective delivery ofH₂ to the skin. In certain embodiments, the hydrogen enrichedcomposition is a beverage in an open container. For topicalcompositions, a composition of the invention can be directlyincorporated into a pharmaceutical grade or cosmetic grade topicalcarrier such as a cream, lotion, foam, paste, or gel. Topicalcompositions containing H₂ can be soaked in, rolled, rubbed on, orsprayed directly onto the skin.

For consumer products designed to be ingested within the human body,e.g., nutraceuticals, e.g., beverages, the acid used in the productionof the composition of the invention must be safely consumable, as withthe edible acids described herein (e.g., malic acid or tartaric acid).The acid used in a composition of the invention to be used in themanufacture of consumer products designed for topical administration maybe any pharmaceutically or cosmetically acceptable acid and itscounterion that are considered “generally regarded as safe” as definedus the U.S. Food and Drug Administration for human and veterinary use.Representative acids include acetic acid, adipic acid, alginic acid,aspartic acid, benzenesulfonic acid, benzoic acid, boric acid, butyricacid, camphoric acid, camphersulfonic acid, cyclopentanepropionic acid,digluconic acid, dodecylsulfric acid, ethanesulfonic acid, glucoheptonicacid, glycerophosphoric acid, hemisulfuric acid, heptonic acid, hexanoicacid, hydrobromic, hydrochloric acid, hydroiodiic acid,2-hydroxy-ethanesulfonic acid, lactobionic acid, lactic acid, lauricacid, lauryl sulfuric acid, malonic acid, methanesulfonic acid,2-naphthalenesulfonic acid, nicotinic acid, nitric acid, oleic acid,palmitic acid, pamoic acid, pectic acid, persulfuric acid,3-phenylpropionic acid, phosphoric acid, picric acid, pivalic acid,propionic acid, stearic acid, sulfuric acid, tartric acid, thiocyanicacid, toluenesulfonic acid, undecanoic acid, valeric acid, theirstereoisomers, all forms of alpha acids (e.g., α-lupulic acid),polycarboxylic acids, a Lewis acid, e.g., AlCl₃, or combinationsthereof. Other such acids are known in the art.

The hydrogen enriched water produced from a composition of the inventionhas a dissolved H₂ concentration between 0.5 mM and 20 mM, e.g., between1 mM and 15 mM, between 1 and 10 mM, between 1 mM and 4 mM, between 1 mMand 3 mM, between 1 mM and 2 mM, between 1.5 mM and 4 mM, or between 2mM and 3 mM, e.g., about 0.5 mM, about 1 mM, about 1.5 mM, about 2 mM,about 3 mM, about 4 mM, about 5 mM, about 6 mM, about 7 mM, about 8 mM,about 9 mM, about 10 mM, about 15 mM, or about 20 mM. In otherembodiments, the concentration is between 1 ppm and 3 ppm, between 2 ppmand 4 ppm, between 3 ppm and 6 ppm, between 4 ppm and 8 ppm, between 5ppm and 10 ppm, between 6 ppm and 12 ppm, or between 5 ppm and 15 ppm.

The acid content of the composition used to enrich the water withhydrogen may be sufficient to maintain a pH of less than 7, e.g., lessthan 6, e.g. between 4-6, while consuming a sufficient amount of themagnesium. A hydrogen enriched composition may also include anutritional supplement, e.g., a magnesium salt, sweetener, flavoringagent, coloring agent, fragrance, essential oil, water-solublelubricant, or a polysaccharide.

EXAMPLES Example 1

In this example, hydrogen enriched water was created by dissolving thefollowing two compositions in separate open containers and monitoringthe evolved hydrogen concentration as a function of time.

Sample composition #1-“F6”—dissolved in 500 mL of water held at 17° C.

80 mg magnesium, −325 mesh, flaked

120 mg tartaric acid, 120 mesh

200 mg malic acid, 120 mesh

200 mg dextrose

6 mg sodium stearyl fumarate

Sample composition #2-“F1”—dissolved in 500 mL of water held at 17° C.

55 mg magnesium, −200 mesh, crushed

25 mg magnesium, −325 mesh, flaked

340 mg malic acid, 60 mesh

160 mg lactose

6 mg sodium stearyl fumarate

The F6 composition containing milled 120 mesh acid particles dissolvedfaster (in approximately 1.75 min) than the F1 composition with larger60 mesh grained acid particles (approximately 3.5 min). If the acids areonly milled to 60 mesh in the F6 composition, the dissolution time ofthe tablet is approximately 3 min. Both the F6 and F1 compositionspassed the minimum pharmaceutical test for friability. Furtherexperimental data using sub-10 micron milled tartaric acid particles inthe F6 composition instead of 120 mesh particles resulted in a tabletdissolution time of 45 seconds. Further, by using dextrose instead oflactose as the binder, the dissolution time per tablet decreased byapproximately 30 second while allowing friability to stay withinacceptable limits.

The hydrogen concentration achieved by the F6 composition after it fullydisintegrated was 9 ppm. For the F1 composition, the hydrogenconcentration after full disintegration was 3.5 ppm. A similarcomposition that did not pass friability testing provided a peakhydrogen concentration of 12 ppm after about 75 seconds. Allconcentration data were an average of approximately 20 individualtablets of each composition.

In a second experiment, the dissolution of a composition containing bothtartaric acid and malic acid (“F35”) with the following ingredients wasinvestigated:

60 mg magnesium, −325 mesh, flaked

90 mg tartaric acid

150 mg malic acid

150 mg dextrose

6 mg sodium stearyl fumarate

In identical water conditions as F1 and F6 (e.g., 500 mL water in opencontainer at 17° C.), the concentration was 5.3 ppm after approximately80-90 s of reaction time. The measured concentration was an average ofapproximately 20 tablets.

Example 2

An exemplary tablet for use in creating a hydrogen enrichedready-to-drink beverage includes the following components:

30 mg −200 mesh magnesium

30 mg −325 mesh magnesium, flaked

90 mg tartaric acid

150 mg malic acid

150 mg dextrose

5.5 mg 2500 mesh stearic acid

Example 3

A tablet for use for producing a hydrogen enriched beverage in a closedcontainer includes the following ingredients:

55 mg −200 mesh magnesium

25 mg −325 mesh magnesium, flaked

310 mg malic acid

100 mg magnesium malate

160 mg lactose

7 mg sodium stearyl fumarate

These ingredients were pressed into a tablet using a hand operatedmechanical tablet press. This tablet, when dissolved in water in anairtight 500 mL container, produces H₂ gas. In a standard soda bottle(500 mL), the H₂ concentration reached 1.6 ppm (0.8 mM) within 15minutes, 4 ppm (2 mM) within 2 hours, and exceeded 6 ppm (3 mM) within12 hours. In a double walled, double gasketed stainless steel bottle,the concentration reached 2.8 ppm (1.4 mM) at 15 minutes, 3.8 ppm (1.9mM) at 1 hour, and exceeded 7 ppm (3.5 mM) at 12 hours. The pH of thefinal solution when the tablet is added to plain water is between 4-6.

When fruit juice, including fruit juices high in pectin such as lemon,lime, apple, and orange, is used as or in addition to the liquid, theconcentration of H₂ in the foam at the top of the liquid can exceed 20ppm (10 mM). An increase in H₂ concentration was also observed withpremixed pectin (Certo®) and psyllium husk.

Example 4

A tablet configured for use in a beverage for producing highconcentration of H₂ includes the following components:

30 mg magnesium

200 mg malic acid

Sufficient amounts of both binding agent and lubricant

These ingredients may be pressed into a suitable tablet shape in atableting die of 9-11 mm in diameter.

Example 5

A tablet configured for use in a cosmetic, shower, or bathtub useinclude the following components:

480 mg magnesium

720 mg tartaric acid

1200 mg malic acid

Sufficient amounts of both binding agent and lubricant to bring thetablet mass to 3600 mg.

These ingredients may be pressed into a suitable tablet shape in atableting die of 24 mm in diameter.

Example 6

A second tablet configured for use in a cosmetic, shower, or bathtub useinclude the following components:

240 mg −325 mesh magnesium

360 mg 80 mesh (or lower) tartaric acid

600 mg 80 mesh (or lower) malic acid

Sufficient amounts of both binding agent and lubricant to bring thetablet mass to 1800 mg.

These ingredients may be pressed into a suitable tablet shape in atableting die of 18 mm in diameter.

Example 7

A tablet configured for use in a beverage or cosmetic spray includes thefollowing components:

80 mg −325 mesh magnesium

120 mg 80 mesh (or lower) tartaric acid

200 mg 80 mesh (or lower) malic acid

Sufficient amounts of both binding agent and lubricant to bring thetablet mass to 600 mg.

These ingredients may be pressed into a suitable tablet shape in atableting die of 12 mm in diameter.

Example 8

A tablet configured for use in a beverage or cosmetic spray includes thefollowing components:

60 mg magnesium

90 mg tartaric acid

200 mg malic acid

Sufficient amounts of both binding agent and lubricant to bring thetablet mass to 4500 mg.

These ingredients may be pressed into a suitable tablet shape in atableting die of 12 mm in diameter.

Example 9

A tablet configured for use exclusively in a cosmetic or beauty sprayincludes the following components:

25-40 mg magnesium

A sufficient amount of acid, in an amount higher than the tablets usedto produce an enriched beverage.

Sufficient amounts of both binding agent and lubricant

These ingredients may be pressed into a suitable tablet shape in atableting die of 9 mm in diameter.

Example 10

An advantage of a tablet comprising finely flaked magnesium particles isthat molecules of H₂ are evolved one at a time. When sufficient acid ispresent, and the mass of magnesium in the tablet is appropriate for thevolume of liquid to be saturated with H₂ (at least 80 mg of magnesiumand 300 mg total acid per 500 mL of liquid), the H₂ will continuouslyevolve, creating bubbles of H₂ first in the picometer size range, beforethey coalesce to nanometer sized bubbles, then micrometer sized bubbles,and then larger bubbles. Nanometer sized bubbles are able to saturate anaqueous solution to a higher level than bubbles of other sizes andtherefore can create a higher pressure of H₂ in the liquid. This isbecause larger bubbles dissipate out of solution, but nanometer sizedbubbles are more stable and the physiochemical properties of thenanometer sized bubbles are different than the individually dissolved H₂molecules, which changes the relation with Henry's Law and the gas'sfugacity coefficient. The increased pressure stops the reaction as perLe Chatelier's principle, leaving sub-micrometer sized magnesium flakessuspended in solution. As the H₂ bubbles coalesce and further dissipate,the pressure of the system drops, and an equal amount of magnesiumreacts to further produce H₂.

This continuous reaction allows for the concentration of H₂ generated tobe greater than 3 ppm when the composition is placed within an opencontainer rather than a sealed bottle, e.g., under 1 atmosphere ofpressure, but deliver a constant replenishment of H₂ to bring it thelocal concentration of H₂ to approximately 9 ppm. The speed of thetablet disintegrating and subsequent reaction of the magnesium and acidcan be accelerated by choosing tablet components, e.g. coatings orbinders, to control the reaction kinetics, with the reaction running tocompletion in no more than 4 minutes, e.g., in the range of 1-2 minutes.

The use of cold water to dissolve compositions of the invention allowsfor the retention of an increased concentration of hydrogen but alsocauses a significant slowing down of the dissolution rate of the tablet,and subsequently the overall hydrogen generation reaction. For example,in water that is just above freezing (1° C.), tablets of the inventiontypically need 4-5 minutes to fully dissolve. Once the water issaturated, though, the dissolved hydrogen is retained for longer in thewater at a higher concentration. The use of hot water to dissolve acomposition of the invention results in a significant increase in thedissolution rate and subsequently faster evolution of hydrogen. Forexample, in hot water, e.g., greater than room temperature, tablets ofthe invention typically fully dissolve is 1 minute or less. However, therate of bubble coalescence increases dramatically with the increasingtemperature, thus reducing the retention time and overall stability ofthe enriched water.

Using current tableting technology and capabilities, the ideal watertemperature range for dissolving a tablet made from a composition of theinvention is between 12-20° C., depending on the final composition ofthe tablet.

Example 11

A composition of the invention, e.g., a tablet, is able to dissolve andproduce a semi-stable supersaturation of H₂ in an open, e.g., ambientpressure, container. Polysaccharides contained within the composition orpresent in the liquid carrier are able to form a boundary layer at thesurface of the liquid. This boundary layer prevents the H₂ gas cloudwhich forms from the dissolution of the composition from quicklydissipating. For example, in a rigid container, the addition of a pHmodifier, e.g., 2 tablespoons of lemon juice (which contains pectin) orvinegar, increases the available concentration of H₂. Use of vinegarresults in a higher concentration of H₂ throughout the liquid. Whenwater and lemon juice are placed in a standard soda bottle madeprimarily of polyethylene terephthalate (PET), the concentration of H₂is increased at the top of the gas cloud by a factor of 6-7x. In an openglass bottle with the same solution of water and lemon juice, theconcentration of H₂ gas produced increases by approximately 20%. Whenpolysaccharides are used, a foam forms on the surface of the liquidwhich includes a higher concentration of H₂ relative to the rest of theliquid.

Open containers are able to quickly create a suspension of magnesiumnanoparticles once the tablet is placed in the container. This increasesthe reaction rate for producing H₂. For example, in a tablet that fullyreacts in 30 to 60 seconds, the bubbles formed at the top of the surfaceaggressively burst and resulted in a measured H₂ concentration of 1.6ppm.

For a composition of the invention, 70-90 seconds is ideal reactionspeed, often reaching 10 ppm of supersaturation within the gas cloud.The measured concentration of H₂ appears to linearly decrease with time,as shown in the data in Table 1, reaching the typical SATP concentrationof 1.6 ppm after 8 minutes of dissolution.

TABLE 1 Measured H₂ concentrations after dissolving a composition of theinvention Time of Dissolution (s) Measured H₂ concertation (ppm) 80-9010 150 6 180 4.5-5 210 3.5-4 300   2.2-2.5 360 1.8 480 1.6

Example 12

In this example, H₂ enhanced water created by dissolving a compositionof the invention, e.g., a tablet, in an open container was transferredinto a sealable swing top glass bottle and allowed to stabilize underpressure upon further dissolution of the composition. When the sealedbottle was opened, the measured concentration of H₂ was 5.3 ppm.

In a further experiment, H₂ enhanced water created by dissolving acomposition of the invention, e.g., a tablet, in an open container wastransferred into a sealable PET soda bottle modified to include apressure gauge for measuring the pressure of the interior of the bottle.As the reaction progressed, that bottle began to pressurize, creating aheadspace within the bottle as H₂ bubbles were formed and subsequentlydissipated. After 5 minutes of reaction, the measured pressure of thebottle was 25 psi, and after 30 minutes of reaction, the measuredpressure of the bottle was 45 psi. At this pressure, the measuredconcentration of H₂ was 2.3 ppm.

The composition in both containers (open and sealed bottle) continued toreact with micrometer particles. As the H₂ coalesced and dissipated, thepressure that had been contained inside the liquid transferred to theheadspace, increasing the pressure in the container. Remarkably, thepressure reached by transferring the open container liquid into the PETbottle reaches and even exceeds the pressure created by dropping atablet into a PET bottle and immediately sealing. The same tabletproduces roughly 35 psi when sealed immediately due to the reactionstopping as per Le Chatelier's principle, thus also confirming thesupersaturation ability of the composition.

Example 13

One variable that exerts control over the production of hydrogen from acomposition of the invention is the mass of magnesium used to react withthe milled acid. The relationship mass of magnesium and dissolvedhydrogen concentration is approximately linear—as the amount ofmagnesium used increases, the amount of hydrogen produced for a fixedmass of acid increases. Table 2 presents hydrogen concentration data fora variety of magnesium masses where the acid was milled to a fine mesh(˜120 mesh) particle size and a dissolution time of approximately 60-75s.

TABLE 2 Measured H₂ concentrations after dissolving a composition of theinvention made with ~120 mesh acid Mass of magnesium (mg) Measured H₂concertation (ppm) 80  9-12 70 N/A 60 4-5 55 3 50 2.6-3 

The effect of milling the acids was also studied by performing laserdiffraction size distribution measurements of the bubbles producedduring the dissolution reaction. Using finely milled acids, thegenerated bubbles exhibited a bimodal distribution, with a first mode ata diameter of approximately 50-60 nm and the second mode at a diameterof 600 nm after compensating for noise. As noted in Example 10,nanometer sized bubbles are able to saturate an aqueous solution to ahigher level than bubbles of other sizes and therefore can create ahigher pressure of H₂ in the liquid, thus confirming the importance ofusing finely milled acids in producing compositions for enriching waterwith hydrogen.

Additional testing in an open container using a tablet made with afinely milled acid produced 70 mL of hydrogen gas out of a theoreticallimit of 80 mL within the first 80-90 seconds. By the second minute ofthe reaction, only 6 mL of hydrogen gas had escaped from the surface ofthe liquid in the open container.

What is claimed is:
 1. A composition comprising: magnesium metal; atleast one acid; and a binding agent; wherein the compositiondisintegrates in less than 5 minutes and produces at least 0.5 mM H₂after contact with 50 mL water in a container at atmospheric pressureand room temperature.
 2. The composition of claim 1, wherein thecomposition passes a pharmaceutical test for friability.
 3. Thecomposition of claim 1, wherein the composition disintegrates in lessthan 2 minutes.
 4. The composition of claim 1, wherein the pH of thewater remains less than 7 for at least 10 minutes after the compositionis contacted by water.
 5. The composition of claim 1, wherein themagnesium metal comprises flakes.
 6. The composition of claim 1, whereinthe magnesium metal comprises −325 mesh flakes.
 7. The composition ofclaim 1, wherein the magnesium metal is crushed.
 8. The composition ofclaim 1, wherein the magnesium metal is of 200 mesh or smaller.
 9. Thecomposition of claim 1, wherein the amount of magnesium metal is 5-500mg.
 10. The composition of claim 1, wherein the at least one acidcomprises an edible acid.
 11. The composition of claim 10, wherein theat least one edible acid is selected from the group consisting of maleicacid, succinic acid, malic acid, fumaric acid, formic acid, citric acid,ascorbic acid, oxalic acid, and tartaric acid, or a mixture thereof. 12.The composition of claim 1, wherein the at least one edible acid istartaric acid.
 13. The composition of claim 1, wherein the at least oneedible acid is malic acid.
 14. The composition of claim 1, wherein theat least one edible acid is of 60 mesh or smaller.
 15. The compositionof claim 1, wherein the at least one acid is a cosmetically orpharmaceutically acceptable acid.
 16. The composition of claim 15,wherein cosmetically or pharmaceutically acceptable acid is acetic acid,adipic acid, alginic acid, aspartic acid, benzenesulfonic acid, benzoicacid, boric acid, butyric acid, camphoric acid, camphersulfonic acid,cyclopentanepropionic acid, digluconic acid, dodecylsulfric acid,ethanesulfonic acid, glucoheptonic acid, glycerophosphoric acid,hemisulfuric acid, heptonic acid, hexanoic acid, hydrobromic,hydrochloric acid, hydroiodiic acid, 2-hydroxy-ethanesulfonic acid,lactobionic acid, lactic acid, lauric acid, lauryl sulfuric acid,malonic acid, methanesulfonic acid, 2-naphthalenesulfonic acid,nicotinic acid, nitric acid, oleic acid, palmitic acid, pamoic acid,pectic acid, persulfuric acid, 3-phenylpropionic acid, phosphoric acid,picric acid, pivalic acid, propionic acid, stearic acid, sulfuric acid,tartric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid,valeric acid, their stereoisomers, all forms of alpha acids (e.g.,α-lupulic acid), polycarboxylic acids, a Lewis acid, or a combinationthereof.
 17. The composition of claim 1, wherein the amount of the atleast one acid is 30-4000 mg.
 18. The composition of claim 1, whereinthe binding agent is mannitol, xylitol, maltose, dextrose, or lactose.19. The composition of claim 1, wherein the binding agent is dextrose.20. The composition of claim 1, wherein the binding agent is lactose.21. The composition of claim 1, further comprising a water-solublelubricant.
 22. The composition of claim 1, where in the water-solublelubricant is selected from sodium stearyl fumarate or steric acid. 23.The composition of claim 1, wherein the water-soluble lubricant issodium stearyl fumarate.
 24. The composition of claim 1, wherein thecontainer is open to the atmosphere.
 25. The composition of claim 1,wherein the container is closed.
 26. The composition of claim 25,wherein the composition maintains a pH of less than 7 at 7 days aftercontact with water.
 27. The composition of claim 1, wherein thecomposition reacts to produce H₂ as it disintegrates when contacted withwater.
 28. The composition of claim 1, wherein the magnesium metal andat least one acid are present in amounts sufficient to produce at least2 mM H₂.
 29. The composition of claim 1, further comprising anutritional supplement.
 30. The composition of claim 29, wherein thenutritional supplement is a magnesium salt.
 31. The composition of claim1, further comprising a sweetener or flavoring agent.
 32. Thecomposition of claim 1, further comprising a coloring agent.
 33. Thecomposition of claim 1, further comprising a fragrance.
 34. Thecomposition of claim 1, further comprising an essential oil.
 35. Thecomposition of claim 1, further comprising a polysaccharide.
 36. Thecomposition of claim 35, wherein the polysaccharide is selected from thegroup consisting of cellulose and its derivatives, starch, apple powder,lemon powder, lime powder, grapefruit powder, psyllium husk, and pectin.37. A composition comprising: magnesium metal; at least onewater-soluble acid; and a binding agent; wherein the compositionproduces at least 0.5 mM H₂ after contact with 50 mL water in acontainer at atmospheric pressure and room temperature and wherein theat least one water-soluble acid has a solubility of at least 0.01 g/mL.38. The composition of claim 37, wherein the composition passes apharmaceutical test for friability.
 39. The composition of claim 37,wherein the composition disintegrates is less than 2 minutes.
 40. Thecomposition of claim 37, wherein the magnesium metal comprises flakes.41. The composition of claim 37, wherein the magnesium metal comprises−325 mesh flakes.
 42. The composition of claim 37, wherein the magnesiummetal is crushed.
 43. The composition of claim 37, wherein the magnesiummetal is of 200 mesh or smaller.
 44. The composition of claim 37,wherein the amount of magnesium metal is 5-500 mg.
 45. The compositionof claim 37, wherein the at least one water-soluble acid has asolubility of at least 0.05 g/mL in water.
 46. The composition of claim37, wherein the at least one water-soluble acid has a solubility of atleast 0.1 g/mL in water.
 47. The composition of claim 37, wherein the atleast one acid water-soluble acid has a solubility of at least 1 g/mL inwater.
 48. The composition of claim 37, wherein the at least one acidwater-soluble acid comprises an edible acid.
 49. The composition ofclaim 48, wherein the at least one water-soluble edible acid is selectedfrom the group consisting of maleic acid, succinic acid, malic acid,fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid, andtartaric acid, or a mixture thereof.
 50. The composition of claim 37,wherein the at least one water-soluble edible acid is tartaric acid. 51.The composition of claim 37, wherein the at least one water-solubleedible acid is malic acid.
 52. The composition of claim 37, wherein theat least one water-soluble edible acid is of 60 mesh or smaller.
 53. Thecomposition of claim 37, wherein the at least one water-soluble acid isa cosmetically or pharmaceutically acceptable acid.
 54. The compositionof claim 53, wherein cosmetically or pharmaceutically acceptable acid isacetic acid, adipic acid, alginic acid, aspartic acid, benzenesulfonicacid, benzoic acid, boric acid, butyric acid, camphoric acid,camphersulfonic acid, cyclopentanepropionic acid, digluconic acid,dodecylsulfric acid, ethanesulfonic acid, glucoheptonic acid,glycerophosphoric acid, hemisulfuric acid, heptonic acid, hexanoic acid,hydrobromic, hydrochloric acid, hydroiodiic acid,2-hydroxy-ethanesulfonic acid, lactobionic acid, lactic acid, lauricacid, lauryl sulfuric acid, malonic acid, methanesulfonic acid,2-naphthalenesulfonic acid, nicotinic acid, nitric acid, oleic acid,palmitic acid, pamoic acid, pectic acid, persulfuric acid,3-phenylpropionic acid, phosphoric acid, picric acid, pivalic acid,propionic acid, stearic acid, sulfuric acid, tartric acid, thiocyanicacid, toluenesulfonic acid, undecanoic acid, valeric acid, theirstereoisomers, all forms of alpha acids (e.g., α-lupulic acid),polycarboxylic acids, a Lewis acid, or a combination thereof.
 55. Thecomposition of claim 37, wherein the amount of the at least onewater-soluble acid is 30-4000 mg.
 56. The composition of claim 37,wherein the binding agent is mannitol, xylitol, maltose, dextrose, orlactose.
 57. The composition of claim 37, wherein the binding agent isdextrose.
 58. The composition of claim 37, wherein the binding agent islactose.
 59. The composition of claim 37, further comprising awater-soluble lubricant.
 60. The composition of claim 37, where in thewater-soluble lubricant is selected from sodium stearyl fumarate orstearic acid.
 61. The composition of claim 37, wherein the water-solublelubricant is sodium stearyl fumarate.
 62. The composition of claim 37,wherein the container is open to the atmosphere.
 63. The composition ofclaim 37, wherein the container is closed.
 64. The composition of claim63, wherein the composition maintains a pH of less than 7 at 7 daysafter contact with water.
 65. The composition of claim 39, wherein thecomposition reacts to produce H₂ as it disintegrates when contacted withwater.
 66. The composition of claim 37, wherein the magnesium metal andat least one water-soluble acid are present in amounts sufficient toproduce at least 2 mM H₂ in 500 mL of water.
 67. The composition ofclaim 37, further comprising a nutritional supplement.
 68. Thecomposition of claim 67, wherein the nutritional supplement is amagnesium salt.
 69. The composition of claim 37, further comprising asweetener or flavoring agent.
 70. The composition of claim 37, furthercomprising a coloring agent.
 71. The composition of claim 37, furthercomprising a fragrance.
 72. The composition of claim 37, furthercomprising an essential oil.
 73. The composition of claim 37, furthercomprising a polysaccharide.
 74. The composition of claim 37, whereinthe polysaccharide is selected from the group consisting of celluloseand its derivatives, starch, apple powder, lemon powder, lime powder,grapefruit powder, psyllium husk, and pectin.
 75. A compositioncomprising: magnesium metal; at least one acid; and a binding agent,wherein the composition produces at least 0.5 mM H₂ after contact with50 mL water in a container at atmospheric pressure and room temperatureand maintains a pH of less than 7 10 minutes after contact.
 76. Thecomposition of claim 75, wherein the composition passes a pharmaceuticaltest for friability.
 77. The composition of claim 75, wherein the pH ofless than 7 is maintained at 30 minutes after contact with water. 78.The composition of claim 75, wherein the pH of less than 7 is maintainedat 1 hour after contact with water.
 79. The composition of claim 75,wherein the magnesium metal comprises flakes.
 80. The composition ofclaim 75, wherein the magnesium metal comprises −325 mesh flakes. 81.The composition of claim 75, wherein the magnesium metal is crushed. 82.The composition of claim 75, wherein the magnesium metal is of 200 meshor smaller.
 83. The composition of claim 75, wherein the amount ofmagnesium metal is 5-500 mg.
 84. The composition of claim 75, whereinthe at least one acid comprises an edible acid.
 85. The composition ofclaim 84, wherein the edible acid is selected from the group consistingof maleic acid, succinic acid, malic acid, fumaric acid, formic acid,citric acid, ascorbic acid, oxalic acid, and tartaric acid, or a mixturethereof.
 86. The composition of claim 75, wherein the at least one acidis tartaric acid.
 87. The composition of claim 75, wherein the at leastone acid is malic acid.
 88. The composition of claim 75, wherein the atleast one acid is of 60 mesh or smaller.
 89. The composition of claim75, wherein the at least one acid is a cosmetically or pharmaceuticallyacceptable acid.
 90. The composition of claim 89, wherein cosmeticallyor pharmaceutically acceptable acid is acetic acid, adipic acid, alginicacid, aspartic acid, benzenesulfonic acid, benzoic acid, boric acid,butyric acid, camphoric acid, camphersulfonic acid,cyclopentanepropionic acid, digluconic acid, dodecylsulfric acid,ethanesulfonic acid, glucoheptonic acid, glycerophosphoric acid,hemisulfuric acid, heptonic acid, hexanoic acid, hydrobromic,hydrochloric acid, hydroiodiic acid, 2-hydroxy-ethanesulfonic acid,lactobionic acid, lactic acid, lauric acid, lauryl sulfuric acid,malonic acid, methanesulfonic acid, 2-naphthalenesulfonic acid,nicotinic acid, nitric acid, oleic acid, palmitic acid, pamoic acid,pectic acid, persulfuric acid, 3-phenylpropionic acid, phosphoric acid,picric acid, pivalic acid, propionic acid, stearic acid, sulfuric acid,tartric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid,valeric acid, their stereoisomers, all forms of alpha acids (e.g.,α-lupulic acid), polycarboxylic acids, a Lewis acid, or a combinationthereof.
 91. The composition of claim 75, wherein the binding agent ismannitol, xylitol, maltose, dextrose, or lactose.
 92. The composition ofclaim 75, further comprising a water-soluble lubricant.
 93. Thecomposition of claim 75, wherein the magnesium metal and acid arepresent in amounts sufficient to produce a pH of between 4 and
 6. 94.The composition of claim 75, wherein the magnesium metal and acid arepresent in amounts sufficient to produce at least 2 mM H₂.
 95. Thecomposition of claim 75, further comprising a nutritional supplement.96. The composition of claim 75, wherein the nutritional supplement is amagnesium salt.
 97. The composition of claim 75, further comprising asweetener or flavoring agent.
 98. The composition of claim 75, furthercomprising a coloring agent.
 99. The composition of claim 75, furthercomprising a fragrance.
 100. The composition of claim 75, furthercomprising an essential oil.
 101. The composition of claim 75, furthercomprising a polysaccharide.
 102. The composition of claim 101, whereinthe polysaccharide is selected from the group consisting of celluloseand its derivatives, e.g. hydroxypropyl methyl cellulose, starch, applepowder, lemon powder, lime powder, grapefruit powder, psyllium husk, andpectin.
 103. A kit comprising a composition of any of claims 1-102 and asealable container capable of holding between 100 mL and 2 L of water.104. The kit of claim 103, wherein the container is double walled. 105.The kit of claim 103, wherein the container is capable of holdingbetween 250-750 mL of water.
 106. A method of producing hydrogen richwater, the method comprising the steps of: contacting a composition ofany one of claims 1-102 with water in a container so that thecomposition disintegrates and the magnesium metal and at least one acidreact to produce H₂.
 107. The method of claim 106, wherein the pH ofless than 7 is sustained for at least 1 hour.
 108. The method of claim106, wherein the pH is 4-6.
 109. The method of claim 106, wherein thewater comprises fruit juice.
 110. The method of claim 106, wherein theconcentration of H₂ is at least 0.5 mM.
 111. A method of administeringhydrogen to a subject, the method comprising providing a subject with acomposition containing hydrogen produced from a composition of any oneof claims 1-102.
 112. The method of claim 111, wherein the compositioncontaining hydrogen is a nutraceutical or topical formulation.
 113. Themethod of claim 111 or 112, wherein the nutraceutical is a beverage.114. A composition enriched with hydrogen, comprising hydrogen dissolvedin a carrier at a concentration of at least 0.5 mM wherein the pH of thecomposition is less than
 7. 115. The composition of claim 114, whereinthe carrier is edible or cosmetic or pharmaceutical grade.
 116. Thecomposition of claim 114 or 115, wherein the carrier is an aqueousliquid, cream, lotion, foam, paste, or gel.
 117. The composition ofclaim 114 being a beverage.
 118. The composition of claim 114, whereinthe maximum concentration of hydrogen is 20 mM.
 119. The composition ofclaim 114, wherein the pH is 4-6.
 120. The composition of claim 114,wherein the pH is 4.6.
 121. The composition of claim 114, furthercomprising a nutritional supplement.
 122. The composition of claim 121,wherein the nutritional supplement comprises magnesium ions.
 123. Thecomposition of claim 114, further comprising a sweetener, flavoringagent, coloring agent, fragrance, essential oil, polysaccharide, bindingagent, or water-soluble lubricant.